SearcharxivSearch

arXiv subjects

A. Ottochian

Publications and source records attributed to A. Ottochian.

2 recordsLinked to original sources

Universal divergenceless scaling between structural relaxation and caged dynamics in glass-forming systems

On approaching the glass transition, the microscopic kinetic unit spends increasing time rattling in the cage of the first neighbours whereas its average escape time, the structural relaxation time $τ_α$, increases from a few picoseconds up to thousands of seconds. A thorough study of the correlation between $τ_α$ and the rattling amplitude, expressed by the Debye-Waller factor (DW), was carried out. Molecular-dynamics (MD) simulations of both a model polymer system and a binary mixture were performed by varying the temperature, the density $ρ$, the potential and the polymer length to consider the structural relaxation as well as both the rotational and the translation diffusion. The simulations evidence the scaling between the $τ_α$ and the Debye-Waller factor. An analytic model of the master curve is developed in terms of two characteristic length scales pertaining to the distance to be covered by the kinetic unit to reach a transition state. The model does not imply $τ_α$ divergences. The comparison with the experiments supports the numerical evidence over a range of relaxation times as wide as about eighteen orders of magnitude. A comparison with other scaling and correlation procedures is presented. The study suggests that the equilibrium and the moderately supercooled states of the glassformers possess key information on the huge slowing-down of their relaxation close to the glass transition. The latter, according to the present simulations, exhibits features consistent with the Lindemann melting criterion and the free-volume model.

cond-mat.soft

Non-gaussian effects in the cage dynamics of polymers

The correlation between the fast cage dynamics and structural relaxation is investigated in a model polymer system. It is shown that the cage vibration amplitude, as expressed by the Debye-Waller factor, and the relaxation time $τ_α$ collapse on a single universal curve with a simple analytic form when the temperature, the density, the chain length and the monomer-monomer interaction potential are changed. For the physical states with the same $τ_α$ coincidence of the mean-square displacement, the intermediate scattering function and the non-Gaussian parameter is observed in a wide time window spanning from the ballistic regime to the onset of the Rouse dynamics driven by the chain connectivity. The role of the non-Gaussian effects is discussed.

physics.flu-dyn